Photo-physics of light amplification in lead halide perovskites

Low temperature solution-processed Organic-Inorganic Hybrid lead-halide Perovskites (OIHPs) nanocrystals (NCs) are new and emerging class of semiconducting materials that possesses high quantum yields (PLQY), large linear and non-linear absorption cross-sections, tunable emission wavelength via faci...

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Main Author: Tay, Eugene Yong Kang
Other Authors: Sum Tze Chien
Format: Thesis-Doctor of Philosophy
Language:English
Published: Nanyang Technological University 2020
Subjects:
Online Access:https://hdl.handle.net/10356/144521
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author Tay, Eugene Yong Kang
author2 Sum Tze Chien
author_facet Sum Tze Chien
Tay, Eugene Yong Kang
author_sort Tay, Eugene Yong Kang
collection NTU
description Low temperature solution-processed Organic-Inorganic Hybrid lead-halide Perovskites (OIHPs) nanocrystals (NCs) are new and emerging class of semiconducting materials that possesses high quantum yields (PLQY), large linear and non-linear absorption cross-sections, tunable emission wavelength via facile halide substitutions/exchanges. These properties make OIHP NCs the ideal candidate for light-emitting applications such as LEDs and lasing. Although preliminary reports showed a consistent trend of low (sub μJcm−2) ASE and lasing thresholds, these NC ensembles suffer from ambient air and moisture attacks, causing degradation and inevitably imposes stringent storage and operation conditions. Furthermore, the main fundamental photo-physics behind its optical gain is still not well understood. Therefore, in this thesis, we focus on (I) proposing a synthetic treatment during the Ligand-Assisted RePrecipitation (LARP) of Methyl Ammonium Lead Bromide (CH3NH3PbBr3) NCs in order to improve its surface passivation, (II) using Photoluminescence (PL) and Time-Resolved Photoluminescence (TR-PL) spectroscopy to characterize its ASE/lasing properties and (III) elucidating its carrier dynamics leading to population inversion and subsequently light amplification via spin-dependent Pump-Probe techniques. Specifically, we show that the bound excitons (BX) in CH3NH3PbBr3 NCs play a crucial role in the formation of zero-spin biexcitons (XX) with low biexciton binding energies (EBXX ~ 20meV), which are responsible for intrinsically spin-unpolarized optical gain mechanisms.
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spelling ntu-10356/1445212023-02-28T23:46:48Z Photo-physics of light amplification in lead halide perovskites Tay, Eugene Yong Kang Sum Tze Chien School of Physical and Mathematical Sciences tzechien@ntu.edu.sg Science::Physics Low temperature solution-processed Organic-Inorganic Hybrid lead-halide Perovskites (OIHPs) nanocrystals (NCs) are new and emerging class of semiconducting materials that possesses high quantum yields (PLQY), large linear and non-linear absorption cross-sections, tunable emission wavelength via facile halide substitutions/exchanges. These properties make OIHP NCs the ideal candidate for light-emitting applications such as LEDs and lasing. Although preliminary reports showed a consistent trend of low (sub μJcm−2) ASE and lasing thresholds, these NC ensembles suffer from ambient air and moisture attacks, causing degradation and inevitably imposes stringent storage and operation conditions. Furthermore, the main fundamental photo-physics behind its optical gain is still not well understood. Therefore, in this thesis, we focus on (I) proposing a synthetic treatment during the Ligand-Assisted RePrecipitation (LARP) of Methyl Ammonium Lead Bromide (CH3NH3PbBr3) NCs in order to improve its surface passivation, (II) using Photoluminescence (PL) and Time-Resolved Photoluminescence (TR-PL) spectroscopy to characterize its ASE/lasing properties and (III) elucidating its carrier dynamics leading to population inversion and subsequently light amplification via spin-dependent Pump-Probe techniques. Specifically, we show that the bound excitons (BX) in CH3NH3PbBr3 NCs play a crucial role in the formation of zero-spin biexcitons (XX) with low biexciton binding energies (EBXX ~ 20meV), which are responsible for intrinsically spin-unpolarized optical gain mechanisms. Doctor of Philosophy 2020-11-11T01:28:17Z 2020-11-11T01:28:17Z 2020 Thesis-Doctor of Philosophy Tay, E. Y. K. (2020). Photo-physics of light amplification in lead halide perovskites. Doctoral thesis, Nanyang Technological University, Singapore. https://hdl.handle.net/10356/144521 10.32657/10356/144521 en This work is licensed under a Creative Commons Attribution-NonCommercial 4.0 International License (CC BY-NC 4.0). application/pdf Nanyang Technological University
spellingShingle Science::Physics
Tay, Eugene Yong Kang
Photo-physics of light amplification in lead halide perovskites
title Photo-physics of light amplification in lead halide perovskites
title_full Photo-physics of light amplification in lead halide perovskites
title_fullStr Photo-physics of light amplification in lead halide perovskites
title_full_unstemmed Photo-physics of light amplification in lead halide perovskites
title_short Photo-physics of light amplification in lead halide perovskites
title_sort photo physics of light amplification in lead halide perovskites
topic Science::Physics
url https://hdl.handle.net/10356/144521
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